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High areal capacity battery electrodes enabled by segregated nanotube networks

Abstract

Increasing the energy storage capability of lithium-ion batteries necessitates maximization of their areal capacity. This requires thick electrodes performing at near-theoretical specific capacity. However, achievable electrode thicknesses are restricted by mechanical instabilities, with high-thickness performance limited by the attainable electrode conductivity. Here we show that forming a segregated network composite of carbon nanotubes with a range of lithium storage materials (for example, silicon, graphite and metal oxide particles) suppresses mechanical instabilities by toughening the composite, allowing the fabrication of high-performance electrodes with thicknesses of up to 800 μm. Such composite electrodes display conductivities up to 1 × 104 S m−1 and low charge-transfer resistances, allowing fast charge-delivery and enabling near-theoretical specific capacities, even for thick electrodes. The combination of high thickness and specific capacity leads to areal capacities of up to 45 and 30 mAh cm−2 for anodes and cathodes, respectively. Combining optimized composite anodes and cathodes yields full cells with state-of-the-art areal capacities (29 mAh cm−2) and specific/volumetric energies (480 Wh kg−1 and 1,600 Wh l−1).

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Data availability

The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.

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Acknowledgements

All authors acknowledge the SFI-funded AMBER research centre (SFI/12/RC/2278) and the Advanced Microscopy Laboratory for the provision of facilities and thank R. Charifou, who performed XRD for the samples. J.N.C. thanks Science Foundation Ireland (SFI, 11/PI/1087), the European Research Council (AdvGr FUTUREPRINT) and the Graphene Flagship (grant agreement no. 785219) for funding. V.N. thanks the European Research Council (SoG 3D2D Print) and Science Foundation Ireland (PIYRA) for funding.

Author information

S.-H.P., P.J.K., J.N.C. and V.N. conceived the project. S.-H.P. and P.J.K. designed materials and experiments. S.-H.P. and P.J.K. fabricated composite electrodes. S.-H.P. performed electrochemical characterization. N.M. performed Raman analysis. S.-H.P., P.J.K., J.C. and R.T. analysed electrochemical data. J.C. and D.D. performed electron microscopic analysis. S.-H.P. and J.C.-F.Z. measured electrical conductivity. C.S.B. and P.M. performed mechanical measurement. S.-H.P. and J.N.C. wrote the manuscript. All authors discussed the results and commented on the manuscript.

Correspondence to Jonathan N. Coleman or Valeria Nicolosi.

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Supplementary Information

Supplementary Figs. 1–28, Supplementary Tables 8, Supplementary Note 1, Supplementary references

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Fig. 1: Fabrication of hierarchical composite electrodes.
Fig. 2: Segregated networks based on different active materials.
Fig. 3: Effect of mechanical reinforcement on achievable thickness.
Fig. 4: Electrochemical characterization of segregated network electrodes with high mass loading.
Fig. 5: Electrochemical performance of full-cell lithium-ion batteries made by pairing 2 μm-Si/7.5 wt%CNT composite anodes with NMC811/0.5 wt%CNT composite cathodes.